AbstractMetal–organic frameworks (MOFs) are exceptional as gas adsorbents but their mechanical properties are poor. We present a successful strategy to improve the mechanical properties along with gas adsorption characteristics, wherein graphene (Gr) is covalently bonded with M/DOBDC (M=Mg²⁺, Ni²⁺, or Co²⁺, DOBDC=2,5‐dioxido‐1,4‐benzene dicarboxylate) MOFs. The surface area of the graphene–MOF composites increases up to 200–300 m² g⁻¹ whereas the CO₂ uptake increases by ca. 3–5 wt % at 0.15 atm and by 6–10 wt % at 1 atm. What is significant is that the composites exhibit improved mechanical properties. In the case of Mg/DOBDC, a three‐fold increase in both the elastic modulus and hardness with 5 wt % graphene reinforcement is observed. Improvement in both the mechanical properties and gas adsorption characteristics of porous MOFs on linking them to graphene is a novel observation and suggests a new avenue for the design and synthesis of porous materials.